Bipolar Tetraarylsilanes as Universal Hosts for Blue,Green, Orange,and White Electrophosphorescence with High Efficiency and Low Efficiency Roll‐Off

A series of tetraarylsilane compounds, namely p‐BISiTPA ( 1 ), m‐BISiTPA ( 2 ), p‐OXDSiTPA ( 3 ), m‐OXDSiTPA ( 4 ), are designed and synthesized by incorporating electron‐donating arylamine and electron‐accepting benzimidazole or oxadiazole into one molecule via a silicon‐bridge linkage mode. Their thermal, photophysical and electrochemical properties can be finely tuned through the different groups and linking topologies. The para‐disposition compounds 1 and 3 display higher glass transition temperatures, slightly lower HOMO levels and triplet energies than their meta‐disposition isomers 2 and 4 , respectively. The silicon‐interrupted conjugation of the electron‐donating and electron‐accepting segments gives these materials the following advantages: i) relative high triplet energies in the range of 2.69–2.73 eV; ii) HOMO/LUMO levels of the compounds mainly depend on the electron‐donating and electron‐accepting groups, respectively; iii) bipolar transporting feature as indicated by hole‐only and electron‐only devices. These advantages make these materials ideal universal hosts for multicolor phosphorescent OLEDs. 1 and 3 have been demonstrated as universal hosts for blue, green, orange and white electrophosphorescence, exhibiting high efficiencies and low efficiency roll‐off. For example, the devices hosted by 1 achieve maximum external quantum efficiencies of 16.1% for blue, 22.7% for green, 20.5% for orange, and 19.1% for white electrophosphorescence. Furthermore, the external quantum efficiencies are still as high as 14.2% for blue, 22.4% for green, 18.9% for orange, and 17.4% for white electrophosphorescence at a high luminance of 1000 cd m^?2. The two‐color, all‐phosphor white device hosted by 3 acquires a maximum current efficiency of 51.4 cd A^?1, and a maximum power efficiency of 51.9 lm W^?1. These values are among the highest for single emitting layer white PhOLEDs reported till now.